Pure praseodymium cerate (Pr₂Ce₂O₇) nanostructures have been successfully synthesized via a facile method, utilizing Pr(NO₃)₃·6H₂O and (NH₄)₂Ce(NO₃)₆ as precursors as well as triethylenetetramine as a new pH regulator. In this study, various complexing agents, different pH regulators and propylene glycol as an esterification agent were utilized to produce Pr₂Ce₂O₇ nanostructures. The as-synthesized praseodymium cerate nanostructures were characterized by energy dispersive X-ray microanalysis (EDX), Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), field emission scanning electron microscopy (FESEM), and UV-vis diffuse reflectance spectroscopy. The obtained results demonstrated that the shape and particle size of the praseodymium cerate depended on the type of complexing agent and pH regulator. To compare the photocatalytic properties of the as-synthesized Pr₂Ce₂O₇ structures, the photocatalytic degradation of methyl orange dye as a model water contaminant was performed.